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An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June-October), aerosol particles reaching 3-5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

54 ENVIRONMENTAL SCIENCES↗

Vertical variation of turbulent entrainment mixing processes in marine stratocumulus clouds using high-resolution digital holography

Marine stratocumulus clouds contribute signi?cantly to the Earth’s radiation budget due to their extensive coverage and high albedo. Yet, subgrid variability in cloud properties such as aerosol concentration, droplet number and precipitation rates lead to considerable errors in global climate models. While these clouds usually have small vertical ex-tent, turbulent entrainment-mixing and precipitation can generate signi?cant variations in droplet number, size and relative dispersion with altitude. In this paper, we analyze turbulent entrainment-mixing processes and the variability in cloud microphysical properties as a function of height within a warm marine stratocumulus cloud layer over the Eastern North Atlantic. We use high resolution airborne holographic measurements and compare them with local turbulence measurements. We ?nd that entrainment-mixing is primarily inhomogeneous near cloud top leading to larger droplet sizes and homogeneous near cloud base leading to smaller droplet sizes. Further analysis of Damk¨ohler number measurements are able to explain the mixing mechanisms at di?erent cloud heights, reinforcing the importance of turbulent mixing and microphysical time scales in deter-mining cloud microphysics.

Desai, Neel↗

Reproductive and leaf litterfall fluxes in forest ecosystem sites globally (1950-2022)

Forest allocation of net primary productivity (NPP) to reproduction is poorly quantified globally, despite its critical role in forest regeneration and a well-supported trade-off with allocation to growth. Although field measurements of total NPP are rare, our work finds that a proxy for reproductive carbon allocation constructed from leaf (L) and reproductive (R) litterfall fluxes, R/(R+L), is strongly correlated with R/NPP, facilitating analysis across a wide range of sites where biometric estimates of NPP are not available (R² = 0.85; Hanbury-Brown et al., 2022, Ward et al., in prep). To investigate relationships between ecosystem-scale reproductive allocation (RA) and climate, soil fertility, and stand age gradients, we conducted a literature search and synthesized 824 observations of annual average leaf and reproductive litterfall fluxes across forest sites globally. The zip file includes 1) a folder Data/ containing the litterfall data ("GlobalForestRA_data.csv") and metadata ("GlobalForestRA_metadata.doc") files. The data file includes geographic coordinates, long-term mean annual temperature and precipitation (1970-2000, extracted from WorldClim2.1), leaf and reproductive litterfall fluxes, sampling interval and protocols, forest characteristics (dominant leaf morphology, information pertaining to forest age and successional stage, and disturbance history) and soil properties (% sand, %silt, %clay, total phosphorus (P), nitrogen (N), cation exchange capacity (CEC) and pH) extracted from SoilGrids250 and from on-site measurements, where available. The metadata file contains information about each variable reported in the data file, including data sources, processing methods, and all references. The Data folder contains two additional files used to create Figure 1; these are described in greater detail in the README.2) R scripts GloalForestRA_analysis.r and GlobalForestRA_SI.r and a folder /Functions used to produce results, figures, and tables in the manuscript Ward et al. (in press)3) a README file describing how the data and R scripts can be used to reproduce statistical results, figures, and tables found in the manuscript. Ward et al. (in press)This repository can also be found at: https://github.com/r-ward/Global_Analysis_ForestRA.Ward, R.E., Zhang-Zheng, H. Aernethy, K., Adu-Bredu, S., Arroyo, L., Bailey, A. et al. (in press). Forest age rivals climate to explain reproductive allocation patterns in forest ecosystems globally. Ecology Letters. Hanbury-Brown, A.R., Ward, R.E. & Kueppers, L.M. (2022). Forest regeneration within Earth system models: current process representations and ways forward. New Phytol., 235, 20–40.Ward et al. (2025), Forest age rivals climate to explain reproductive allocation patterns in forest ecosystems globally, in prep.

54 ENVIRONMENTAL SCIENCES↗

Global distribution, formation and fate of mineral‐associated soil organic matter under a changing climate: A trait‐based perspective

Abstract Soil organic matter (SOM) is the largest actively cycling reservoir of terrestrial carbon (C), and the majority of SOM in Earth's mineral soils (~65%) is mineral‐associated organic matter (MAOM). Thus, the formation and fate of MAOM can exert substantial influence on the global C cycle. To predict future changes to Earth's climate, it is critical to mechanistically understand the processes by which MAOM is formed and decomposed, and to accurately represent this process‐based understanding in biogeochemical and Earth system models. In this review, we use a trait‐based framework to synthesize the interacting roles of plants, soil micro‐organisms, and the mineral matrix in regulating MAOM formation and decomposition. Our proposed framework differentiates between plant and microbial traits that influence total OM inputs to the soil (‘feedstock traits’) versus traits that influence the proportion of OM inputs that are ultimately incorporated into MAOM (‘MAOM formation traits’). We discuss how these feedstock and MAOM formation traits may be altered by warming, altered precipitation and elevated carbon dioxide. At a planetary scale, these feedstock and MAOM formation traits help shape the distribution of MAOM across Earth's biomes, and modulate biome‐specific responses of MAOM to climate change. We leverage a global synthesis of MAOM measurements to provide estimates of the total amount of MAOM‐C globally (~840–1540 Pg C; 34%–51% of total terrestrial organic C), and its distribution across Earth's biomes. We show that MAOM‐C concentration is highest in temperate forests and grasslands, and lowest in shrublands and savannas. Grasslands and croplands have the highest proportion of soil organic carbon (SOC) in the MAOM fraction (i.e. the MAOM‐C:SOC ratio), while boreal forests and tundra have the lowest MAOM‐C:SOC ratio. Drawing on our trait framework, we then review experimental data and posit the effects of climate change on MAOM pools in different biomes. We conclude by discussing how MAOM is integrated into soil C models, and how feedstock and MAOM formation traits may be included in these models. We also summarize the projected fate of MAOM under climate change scenarios (Representative Concentration Pathways 4.5 and 8.5) and discuss key model uncertainties. Read the free Plain Language Summary for this article on the Journal blog.

54 ENVIRONMENTAL SCIENCES↗

A Surface Radiation Balance Dataset from Siple Dome in West Antarctica for Atmospheric and Climate Model Evaluation

Abstract A field campaign at Siple Dome in West Antarctica during the austral summer 2019/20 offers an opportunity to evaluate climate model performance, particularly cloud microphysical simulation. Over Antarctic ice sheets and ice shelves, clouds are a major regulator of the surface energy balance, and in the warm season their presence occasionally induces surface melt that can gradually weaken an ice shelf structure. This dataset from Siple Dome, obtained using transportable and solar-powered equipment, includes surface energy balance measurements, meteorology, and cloud remote sensing. To demonstrate how these data can be used to evaluate model performance, comparisons are made with meteorological reanalysis known to give generally good performance over Antarctica (ERA5). Surface albedo measurements show expected variability with observed cloud amount, and can be used to evaluate a model’s snowpack parameterization. One case study discussed involves a squall with northerly winds, during which ERA5 fails to produce cloud cover throughout one of the days. A second case study illustrates how shortwave spectroradiometer measurements that encompass the 1.6- μ m atmospheric window reveal cloud phase transitions associated with cloud life cycle. Here, continuously precipitating mixed-phase clouds become mainly liquid water clouds from local morning through the afternoon, not reproduced by ERA5. We challenge researchers to run their various regional or global models in a manner that has the large-scale meteorology follow the conditions of this field campaign, compare cloud and radiation simulations with this Siple Dome dataset, and potentially investigate why cloud microphysical simulations or other model components might produce discrepancies with these observations. significance statement Antarctica is a critical region for understanding climate change and sea level rise, as the great ice sheets and the ice shelves are subject to increasing risk as global climate warms. Climate models have difficulties over Antarctica, particularly with simulation of cloud properties that regulate snow surface melting or refreezing. Atmospheric and climate-related field work has significant challenges in the Antarctic, due to the small number of research stations that can support state-of-the-art equipment. Here we present new data from a suite of transportable and solar-powered instruments that can be deployed to remote Antarctic sites, including regions where ice shelves are most at risk, and we demonstrate how key components of climate model simulations can be evaluated against these data.

54 ENVIRONMENTAL SCIENCES↗

Science Plan for the Deployment of the Third ARM Mobile Facility to the Southeastern United States at the Bankhead National Forest, Alabama (AMF3 BNF)

In 2018, the U.S. Department of Energy (DOE) held a workshop for the Atmospheric Radiation Measurement (ARM) (Mather and Voyles 2013) user facility to discuss critical climate challenges and locations where key ARM Mobile Facility (AMF) observational assets could impact Earth system modeling (ESM). As an outcome, the southeast United States (SE U.S.) was identified as a high-priority region to target climate-process studies that promote a deeper understanding of the climate system and bolster ARM interactions with the community to drive ESM advancement. The DOE ARM user facility is a globally recognized leader in deploying and operating strategically located observation sites around the world for studying the properties of aerosols and clouds and their interaction with radiation, precipitation, and the Earth’s surface. In partnering with the DOE Atmospheric System Research (ASR) program, ARM solicited a multi-agency Site Science Team approach to provide input and close interaction with ARM management towards a successful SE U.S. deployment of the ARM third Mobile Facility (AMF3) (Miller et al. 2016). These efforts included identifying key locations, science drivers and instruments, and measurement strategies to address the wider climate-process needs and ESM improvement. Community input served a vital role in establishing, refining, and informing the relevant drivers and decisions regarding this AMF3 deployment. The team has identified Northern Alabama (N. AL) as regionally representative to unlock the key opportunities that will improve our understanding and model representation of aerosol, cloud, and land-surface processes and their couplings in the SE U.S. A defining aspect of the AMF3 deployment is its commitment to long-term (anticipated five-year) observations to mitigate potential seasonal-to-annual variability that often limits appropriate attribution of phenomena to local or larger-scale processes. The proposed location may leverage nearby surface networks and multi-agency and partner assets to enrich this multi-year deployment. One motivation is to understand the role of spatiotemporal variability (thermodynamic, land-surface) across aspects of the climate system, with our AMF3 team anticipating future demands on characterizing the relationships between local-to-regional cloud development and surface processes across a diverse patchwork of natural, managed, and urban landscapes as found throughout the N. AL regions. The main site targets an intact, representative, forested region – the Bankhead National Forest (BNF) – underscoring further team commitment to regionally important land-atmosphere two-way interactive studies “from the canopy to the clouds”, with enhanced tower instrumentation augmenting traditional ARM capabilities adjacent to this site. Multiple supplemental sites will also be distributed across this region, prioritizing added needs for biodiversity. Anticipated high-priority cloud science themes will target N. AL as a regional SE U.S. hotbed for high-impact weather, convective cloud onset, and shallow-to-deep cloud transitioning. Anticipated aerosol drivers will focus on chemical processes that control the evolution of organic aerosol, the seasonality and spatial distribution of water vapor and particle-phase water, and its role on aerosol optical properties. Anticipated land-atmosphere drivers consider the two-way feedbacks between surface influence on aerosols, clouds, and precipitation properties and the associated radiative impacts on plant physiology and canopy-scale fluxes. Emphasis will include the study of the impact of surface processes on aerosols via precursor emission, and on clouds via moisture flux and thermal development.

54 ENVIRONMENTAL SCIENCES↗

Science Plan for the Deployment of the Third ARM Mobile Facility to the Southeastern United States at the Bankhead National Forest, Alabama (AMF3 BNF)

In 2018, the U.S. Department of Energy (DOE) held a workshop for the Atmospheric Radiation Measurement (ARM) (Mather and Voyles 2013) user facility to discuss critical climate challenges and locations where key ARM Mobile Facility (AMF) observational assets could impact Earth system modeling (ESM). As an outcome, the southeast United States (SE U.S.) was identified as a high-priority region to target climate-process studies that promote a deeper understanding of the climate system and bolster ARM interactions with the community to drive ESM advancement. The DOE ARM user facility is a globally recognized leader in deploying and operating strategically located observation sites around the world for studying the properties of aerosols and clouds and their interaction with radiation, precipitation, and the Earth’s surface. In partnering with the DOE Atmospheric System Research (ASR) program, ARM solicited a multi-agency Site Science Team approach to provide input and close interaction with ARM management towards a successful SE U.S. deployment of the ARM third Mobile Facility (AMF3) (Miller et al. 2016). These efforts included identifying key locations, science drivers and instruments, and measurement strategies to address the wider climate-process needs and ESM improvement. Community input served a vital role in establishing, refining, and informing the relevant drivers and decisions regarding this AMF3 deployment. The team has identified Northern Alabama (N. AL) as regionally representative to unlock the key opportunities that will improve our understanding and model representation of aerosol, cloud, and land surface processes and their couplings in the SE U.S. A defining aspect of the AMF3 deployment is its commitment to long-term (anticipated five-year) observations to mitigate potential seasonal-to-annual variability that often limits appropriate attribution of phenomena to local or larger-scale processes. The proposed location may leverage nearby surface networks and multi-agency and partner assets to enrich this multi-year deployment. One motivation is to understand the role of spatiotemporal variability (thermodynamic, land-surface) across aspects of the climate system, with our AMF3 team anticipating future demands on characterizing the relationships between local-to-regional cloud development and surface processes across a diverse patchwork of natural, managed, and urban landscapes as found throughout the N. AL regions. The main site targets an intact, representative, forested region – the Bankhead National Forest (BNF) – underscoring further team commitment to regionally important land atmosphere two-way interactive studies “from the canopy to the clouds”, with enhanced tower instrumentation augmenting traditional ARM capabilities adjacent to this site. Multiple supplemental sites will also be distributed across this region, prioritizing added needs for biodiversity. Anticipated high-priority cloud science themes will target N. AL as a regional SE U.S. hotbed for high-impact weather, convective cloud onset, and shallow to-deep cloud transitioning. Anticipated aerosol drivers will focus on chemical processes that control the evolution of organic aerosol, the seasonality and spatial distribution of water vapor and particle-phase water, and its role on aerosol optical properties. Anticipated land atmosphere drivers consider the two-way feedbacks between surface influence on aerosols, clouds, and precipitation properties and the associated radiative impacts on plant physiology and canopy-scale fluxes. Emphasis will include the study of the impact of surface processes on aerosols via precursor emission, and on clouds via moisture flux and thermal development.

Doppler lidar, aerosols, convection↗

Dryland feedbacks to future climate change: how species mortality and replacement will affect coupled biogeochemical cycles and energy balance (Final Technical Report)

The overall goal of the dryland climate manipulation experiment is to improve our understanding and ability to forecast dryland responses to increasing temperatures and altered precipitation regimes. Drylands cover over 40% of Earth’s terrestrial surface and are predicted to increase in size 11-23% by 2100. Yet our understanding of this vast biome, which exchanges enormous amounts of CO 2 and energy with the atmosphere, is exceedingly poor. This project aims to transform and improve that understanding in order to reduce uncertainty and increase the confidence with which we can make global predictions of future climate. We focus on both above- and belowground processes, and explore temperature controls over critical aspects of carbon and nutrient cycling for dryland plants, soil, and microbes. We have 60 climate manipulation plots where plants (from above the canopy) and soils are warmed using infrared lamps and where precipitation has been altered using targeted watering regimes. We have measured myriad aspects of plant physiology, morphology, carbon exchange, energy exchange, and phenology, as well as analogous climate-induced changes to biological soil crusts and soil microbial communities. Our goals are to investigate temperature responses and acclimation potential of dryland plant and soil processes. Concurrent soil incubation experiments complement the in-situ soil warming component and enable more controlled mechanistic investigations of temperature response on microbial function. Automated soil CO 2 efflux chambers within the plots provide phenomenal opportunity to improve our understanding of dryland CO 2 exchange with the atmosphere and are coupled with plant CO 2 exchange measurements. The project has been exceptionally successful, with 35 peer-reviewed publications (and more in review), including in high-profile journals such as Nature Climate Change and PNAS. We have given over fifty presentations on the work and it has been featured in many high-profile media outlets, such as Discover Magazine and on NPR.

54 ENVIRONMENTAL SCIENCES↗

Observational constraints on wet and dry deposition of black carbon to land surfaces (Final Report)

This project focused on providing observational constraints on dry deposition of black carbon and aerosol particles, and the extent to which wet and dry deposition impacts the lifetime of aerosols in the atmosphere. The proposed work tackled the following questions: To what extent dry versus wet deposition controls the removal of BC from the atmosphere, and thus atmospheric BC concentrations? Is BC dry deposition controlled by the same processes as non-refractory aerosol dry deposition? We successfully made eddy covariance flux measurements at the DOE Southern Great Plains site of size-resolved aerosol number fluxes with an ultra high sensitivity aerosol spectrometer (UHSAS) and of black carbon mass and number fluxes using a single particle soot photometer (SP2). We also collected precipitation samples for off-line measurement of rBC using a wet deposition collector. Using these measurements, we identified that wet deposition was the dominant control for black carbon lifetime, but that dry deposition was poorly constrained in models. We developed a new parameterization for particle dry deposition, and applied it to global models to demonstrate the importance of dry deposition in air pollution and radiative effect estimates.

54 ENVIRONMENTAL SCIENCES↗

A biogenic secondary organic aerosol source of cirrus ice nucleating particles

Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46°C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L –1 . Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exposing Process‐Level Biases in a Global Cloud Permitting Model With ARM Observations

The emergence of global convective‐permitting models (GCPMs) represents a significant advancement in climate modeling, offering improved representation of deep convection and complex precipitation patterns. In this study, we evaluate the performance of the Simple Cloud‐Resolving E3SM Atmosphere Model (SCREAM) using its doubly periodic configuration (DP‐SCREAM) against large eddy simulations and modern observational data sets from the Atmospheric Radiation Measurement program. We introduce several new transitional cloud regime cases, such as the transition from shallow to deep convection and from stratocumulus to cumulus, as well as cold‐air outbreak scenarios. The results reveal both strengths and limitations of SCREAM, particularly in the accurate simulation of cloud transitions and midlevel convection, with varying degrees of sensitivity to horizontal and vertical resolution. Despite improvements at higher resolutions, key biases remain, including the abrupt transition from shallow to deep convection and the lack of congestus clouds. These findings underscore the need for further refinement in turbulence parameterizations and vertical grid resolution in GCPMs.

Bogenschutz, Peter A. [Lawrence Livermore National↗

Revolutionizing observations and predictability of Arctic system dynamics through next-generation dense, heterogeneous and intelligent wireless sensor networks with embedded AI

The Arctic region is a complex and dynamic system, where changes in temperature and partitioning between water in solid, liquid and vapor phase are fundamentally reshaping hydro-biogeochemical fluxes from the bedrock to the atmosphere. The increasing temperature and frequency of extreme heat, precipitation and fire events (Wang et al., 2017; Meredith et al., 2019) have critical consequences for the Arctic ecosystems and people, as well as for the global climate system. Although many observational and remote sensing activities have been on-going, detailed ecosystem processes – particularly related to controls on and impacts of permafrost thaw – are difficult to detect or measure. To improve the understanding and prediction of these extreme events and their consequences, we need a revolution in the way we collect ground-based observations from hillslope to pan-Arctic scales and couple them with satellite imagery and models to deliver rich, actionable, and scale-appropriate data.

54 ENVIRONMENTAL SCIENCES↗

Unveiling four decades of intensifying precipitation from tropical cyclones using satellite measurements

Increases in precipitation rates and volumes from tropical cyclones (TCs) caused by anthropogenic warming are predicted by climate modeling studies and have been identified in several high intensity storms occurring over the last half decade. However, it has been difficult to detect historical trends in TC precipitation at time scales long enough to overcome natural climate variability because of limitations in existing precipitation observations. We introduce an experimental global high-resolution climate data record of precipitation produced using infrared satellite imagery and corrected at the monthly scale by a gauge-derived product that shows generally good performance during two hurricane case studies but estimates higher mean precipitation rates in the tropics than the evaluation datasets. General increases in mean and extreme rainfall rates during the study period of 1980–2019 are identified, culminating in a 12–18%/40-year increase in global rainfall rates. Overall, all basins have experienced intensification in precipitation rates. Increases in rainfall rates have boosted the mean precipitation volume of global TCs by 7–15% over 40 years, with the starkest rises seen in the North Atlantic, South Indian, and South Pacific basins (maximum 59–64% over 40 years). In terms of inland rainfall totals, year-by-year trends are generally positive due to increasing TC frequency, slower decay over land, and more intense rainfall, with an alarming increase of 81–85% seen from the strongest global TCs. As the global trend in precipitation rates follows expectations from warming sea surface temperatures (11.1%/°C), we hypothesize that the observed trends could be a result of anthropogenic warming creating greater concentrations of water vapor in the atmosphere, though retrospective studies of TC dynamics over the period are needed to confirm.

54 ENVIRONMENTAL SCIENCES↗

SPARTAN and IMPROVE Comparison Experiment (SPICE) Interim Campaign Report

SPICE (the SPARTAN and IMPROVE Comparison Experiment) aims to obtain and quantify comparisons between aerosol PM 2.5 mass concentration measurements from the University of Oklahoma (OU) Surface Particulate Matter Network (SPARTAN) station and the U.S. Environmental Protection Agency (EPA) Interagency Monitoring of Protected Visual Environments (IMPROVE) station hosted by the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) User Facility at ARM’s Southern Great Plains (SGP) observatory in Oklahoma. Aerosols—both natural and anthropogenic—affect human populations in multiple ways. Much of ARM’s research focuses on how aerosols influence weather and climate through their optical and radiative effects, as well as their impacts on clouds and precipitation. However, aerosols also pose direct risks to humans and other organisms through inhalation, with the severity of health impacts depending on particle size, chemical composition, and duration of exposure. The IMPROVE network was established by the U.S. EPA to monitor air quality, including visible clarity as well as total and chemically speciated aerosol mass concentrations. The ARM SGP site hosts the IMPROVE SOGP station. Separately, the SPARTAN network operates a globally distributed set of stations similar to IMPROVE but with an emphasis on remote deployment and semi-autonomous operation for use beyond the borders of the United States (IMPROVE only operates within the U.S.). The University of Oklahoma operates a SPARTAN station. To establish confidence in the OU SPARTAN instrumentation and measurement protocol relative to the EPA-certified IMPROVE station, the OU SPARTAN station is currently deployed at SGP in close proximity to the IMPROVE SOGP station. The SPICE campaign was envisioned as a contiguous calendar-year effort for 2025 to capture seasonal variation in mass loading as well as composition. However, independent of the SPICE campaign, the SPARTAN network adopted a new filter construction part-way through the year, interrupting our contiguous data set. Thus, to obtain a contiguous data set with a uniform consistent configuration, SPICE desires an extension through 2026.

54 ENVIRONMENTAL SCIENCES↗

Ice Nucleating Particles, Aerosols and Clouds over the Higher Latitude Southern Ocean

Improved understanding of aerosol-cloud-precipitation interactions is a key goal of the DOE-ASR program. Ice Nucleating Particles (INPs) are rare aerosol particles that trigger ice formation in clouds. By doing so they may initiate precipitation in clouds, and this impacts cloud lifetime. Nowhere may the role of INPs be manifested so dramatically as in the Southern Ocean (SO). This vast region was the focus of the DOE-ARM MARCUS (Measurement of Aerosols, Radiation and CloUds over the Southern Oceans) and MICRE (Macquarie Island Cloud and Radiation Experiment) campaigns. In the SO, a deficit of INPs has been a leading hypothesis for why liquid clouds persist, which underlays the bias of global climate models in predicting excess shortwave radiation reaching the ocean surface between 55°S and Antarctica. In this study, we used the 6-month acquisition of INP data on four MARCUS cruises from Hobart, Tasmania, to Antarctica, and the single-location full annual INP cycle observed in MICRE, to gain a holistic, quantitative picture of the INP number concentrations as a function of temperature and their variability over SO latitudes from 43°S to Antarctica. Augmenting initial processing of filter collections of aerosol particles during MARCUS and MICRE, additional freezing studies following thermal treatment (to removes INPs associated with microbes) and peroxide treatment (to remove all organics), as well as ionic chemistry and total organic carbon analysis, were applied to samples to improve time and space resolution, and differentiate marine from terrestrial contributions. We also performed Next Generation Sequencing to determine that bacterial composition can tag periods of enhanced and degraded marine organic INPs and the relative lack of occurrence of land-sourced bio-particles. Through these and other analyses, INP data were categorized into representative source types (e.g., marine versus terrestrially-influenced). The products of our analyses are being used to parameterize ice formation for use in numerical modeling studies to determine if, and when, ocean-derived INPs control the microphysical composition and radiative balance of SO clouds in a manner not presently captured by global models. The specific objectives and approaches proposed were largely accomplished, including: 1) Additional and value-added chemical and biological analyses of archived samples of aerosols were completed to categorize and quantify INP types and concentrations over the SO. 2) Analyses were completed to place INP data in meteorological and aerosol context. 3) Sea spray aerosol INPs were demonstrated to dominate the SO region in all but episodic events. 4) New parameterizations for INP sources relevant to the SO were constructed. 5) Collaborative modeling studies demonstrating the crucial role of INPs in determining cloud radiative and precipitation properties were conducted with MARCUS and MICRE partners. Collaborative publication submissions in this regard ensued within the two year study. This work will advance the science of interactions of aerosols, clouds and precipitation, to improve their representation in regional and global climate models. Results have informed representation of primary ice crystal nucleation, give inference to the role of secondary processes, and improve investigations of aerosol influences on clouds via ice nucleation over SO high latitudes and similar vast ocean regions. Application will improve representation of such interactions for clouds in both regional and global climate models. The data base and analyses methods applied will continue to serve research studies in the future.

58 GEOSCIENCES↗

EPCAPE-Dalhousie Field Campaign Report

This project supported the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), which aimed to characterize the extent, radiative properties, aerosol interactions, and precipitation of stratocumulus clouds in the Eastern Pacific coastal region of La Jolla, California. Given the frequent anthropogenic aerosols emitted into this region, characterization of this important coastal cloud region and the aerosol impact on the cloud characteristics will improve the understanding of aerosol indirect effects and its representation in global climate models. This specific project deployed the fog droplet monitor (FM-120, Droplet Measurement Technologies) at the Scripps Institution of Oceanography’s Mt. Soledad site from 16 February 2023 to 15 February 2024. This instrument measured droplet number size spectra between 2 and 50 microns, from which droplet number concentration, liquid water content, and effective diameter were calculated. These measurements will be used to characterize the seasonal variability of clouds at Mt. Soledad and investigate differences in cloud properties under regional polluted and clean marine conditions. The collected data will soon be posted as part of the digital collection for EPCAPE data hosted by the University of California, San Diego (Russell et al. 2023).

54 ENVIRONMENTAL SCIENCES↗

Using machine learning to derive cloud condensation nuclei number concentrations from commonly available measurements

Cloud condensation nuclei (CCN) number concentrations are an important aspect of aerosol–cloud interactions and the subsequent climate effects; however, their measurements are very limited. We use a machine learning tool, random decision forests, to develop a random forest regression model (RFRM) to derive CCN at 0.4 % supersaturation ([CCN0.4]) from commonly available measurements. The RFRM is trained on the long-term simulations in a global size-resolved particle microphysics model. Using atmospheric state and composition variables as predictors, through associations of their variabilities, the RFRM is able to learn the underlying dependence of [CCN0.4] on these predictors, which are as follows: eight fractions of PM 2.5 (NH 4 , SO 4 , NO 3, secondary organic aerosol (SOA), black carbon (BC), primary organic carbon (POC), dust, and salt), seven gaseous species (NO x , NH 3 , O 3 , SO 2 , OH, isoprene, and monoterpene), and four meteorological variables (temperature (T), relative humidity (RH), precipitation, and solar radiation). The RFRM is highly robust: it has a median mean fractional bias (MFB) of 4.4 % with ≈96.33 % of the derived [CCN0.4] within a good agreement range of -60% 2.5 speciation (NH 4 , SO 4 , NO 3 , and organic carbon (OC)), NO x , O 3 , SO 2 , T, and RH, as well as [CCN0.4] are available. We modify, optimize, and retrain the developed RFRM to make predictions from 19 to 9 of these available predictors. This retrained RFRM (RFRM-ShortVars) shows a reduction in performance due to the unavailability and sparsity of measurements (predictors); it captures the [CCN0.4] variability and magnitude at SGP with ≈67.02 % of the derived values in the good agreement range. This work shows the potential of using the more commonly available measurements of PM 2.5 speciation to alleviate the sparsity of CCN number concentrations' measurements.

54 ENVIRONMENTAL SCIENCES↗

Benchmarking Simulated Precipitation Variability Amplitude across Time Scales

Here, objective performance metrics that measure precipitation variability across time scales from subdaily to interannual are presented and applied to Historical simulations of Coupled Model Intercomparison Project phase 5 and 6 (CMIP5 and CMIP6) models. Three satellite-based precipitation estimates (IMERG, TRMM, and CMORPH) are used as reference data. We apply two independent methods to estimate temporal variability of precipitation and compare the consistency in their results. The first method is derived from power spectra analysis of 3-hourly precipitation, measuring forced variability by solar insolation (diurnal and annual cycles) and internal variability at different time scales (subdaily, synoptic, subseasonal, seasonal, and interannual). The second method is based on time averaging and facilitates estimating the seasonality of subdaily variability. Supporting the robustness of our metric, we find a near equivalence between the results obtained from the two methods when examining simulated-to-observed ratios over large domains (global, tropics, extratropics, land, or ocean). Additionally, we demonstrate that our model evaluation is not very sensitive to the discrepancies between observations. Our results reveal that CMIP5 and CMIP6 models in general overestimate the forced variability while they underestimate the internal variability, especially in the tropical ocean and higher-frequency variability. The underestimation of subdaily variability is consistent across different seasons. The internal variability is overall improved in CMIP6, but remains underestimated, and there is little evidence of improvement in forced variability. Increased horizontal resolution results in some improvement of internal variability at subdaily and synoptic time scales, but not at longer time scales.

54 ENVIRONMENTAL SCIENCES↗